Phase engineering has a profound effect on the chemical bonding and electric configuration, which play significant roles in regulating the activities of catalysts. The metallic phases of transition-metal dichalcogenides (TMDs) have been proposed to show more excellent performance in electrocatalysis over their semiconductor phase; however, the controllable phase engineering for these compounds remains a challenge. In this work, filmlike 1T′ MoTe 2 (F-1T′ MoTe 2 ), filmlike 1T′/ 2H MoTe 2 , porous 1T′ MoTe 2 , small granular 1T′ MoTe 2 , and large granular 1T′ MoTe 2 were successfully synthesized on a flexible carbon cloth (CC) substrate with 3D network structure by chemical vapor deposition (CVD). The high activity of the assynthesized F-1T′ MoTe 2 /CC electrode for HER in 1 M H 2 SO 4 solution was demonstrated by the small onset overpotential of −230.7 mV, a low Tafel slope of 127.1 mV dec −1 , and robust electrochemical durability. The enhanced electrocatalytic activity and stability of F-1T′ MoTe 2 /CC benefit from excellent catalytically active sites and remarkable conductivity of the F-1T′ MoTe 2 . The results demonstrate an efficient route to designing and constructing metallic-phase TMD catalysts for high-performance electrocatalytic devices. KEYWORDS: 1T′ MoTe 2 , carbon cloth, CVD, H 2 SO 4 , HER